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Title: Probing the microhydration of metal carbonyls: a photoelectron velocity-map imaging spectroscopic and theoretical study of Ni(CO)3(H2O)n–

Abstract

A series of microhydrated nickel carbonyls, Ni(CO)3(H2O)n– (n = 0–4), are prepared via a laser vaporization supersonic cluster source in the gas phase and identified by mass-selected photoelectron velocity-map imaging spectroscopy and quantum chemical calculations. Vertical detachment energies for the n = 1–4 anions are measured from the photoelectron spectra to be 1.429 ± 0.103, 1.698 ± 0.090, 1.887 ± 0.080, and 2.023 ± 0.074 eV, respectively. The C–O stretching vibrational frequencies in the corresponding neutral clusters are determined to be 1968, 1950, 1945, and 1940 cm–1 for n = 1–4, respectively, which are characteristic of terminal CO. It is determined that the hydrogen atom of the first water molecule is bound to the nickel center. Addition of a second water molecule prefers solvation at the carbonyl terminal. Spectroscopy combined with theory suggests that the solvation of nickel tricarbonyl is dominated by a water-ring network. Here, the present findings would have important implications for the fundamental understanding of the multifaceted mechanisms of the multibody interaction of water and carbon monoxide with transition metals.

Authors:
 [1];  [1];  [1];  [1];  [2];  [1]
+ Show Author Affiliations
  1. Chinese Academy of Sciences, Dalian (People's Republic of China)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
OSTI Identifier:
1464132
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP
Additional Journal Information:
Journal Volume: 18; Journal Issue: 38; Related Information: © 2016 the Owner Societies.; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Xie, Hua, Zou, Jinghan, Kong, Xiangtao, Zhang, Weiqing, Ahmed, Musahid, and Jiang, Ling. Probing the microhydration of metal carbonyls: a photoelectron velocity-map imaging spectroscopic and theoretical study of Ni(CO)3(H2O)n–. United States: N. p., 2016. Web. doi:10.1039/c6cp05035b.
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Xie, Hua, Zou, Jinghan, Kong, Xiangtao, Zhang, Weiqing, Ahmed, Musahid, & Jiang, Ling. Probing the microhydration of metal carbonyls: a photoelectron velocity-map imaging spectroscopic and theoretical study of Ni(CO)3(H2O)n–. United States. https://doi.org/10.1039/c6cp05035b
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Xie, Hua, Zou, Jinghan, Kong, Xiangtao, Zhang, Weiqing, Ahmed, Musahid, and Jiang, Ling. Fri . "Probing the microhydration of metal carbonyls: a photoelectron velocity-map imaging spectroscopic and theoretical study of Ni(CO)3(H2O)n–". United States. https://doi.org/10.1039/c6cp05035b. https://www.osti.gov/servlets/purl/1464132.
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@article{osti_1464132,
title = {Probing the microhydration of metal carbonyls: a photoelectron velocity-map imaging spectroscopic and theoretical study of Ni(CO)3(H2O)n–},
author = {Xie, Hua and Zou, Jinghan and Kong, Xiangtao and Zhang, Weiqing and Ahmed, Musahid and Jiang, Ling},
abstractNote = {A series of microhydrated nickel carbonyls, Ni(CO)3(H2O)n– (n = 0–4), are prepared via a laser vaporization supersonic cluster source in the gas phase and identified by mass-selected photoelectron velocity-map imaging spectroscopy and quantum chemical calculations. Vertical detachment energies for the n = 1–4 anions are measured from the photoelectron spectra to be 1.429 ± 0.103, 1.698 ± 0.090, 1.887 ± 0.080, and 2.023 ± 0.074 eV, respectively. The C–O stretching vibrational frequencies in the corresponding neutral clusters are determined to be 1968, 1950, 1945, and 1940 cm–1 for n = 1–4, respectively, which are characteristic of terminal CO. It is determined that the hydrogen atom of the first water molecule is bound to the nickel center. Addition of a second water molecule prefers solvation at the carbonyl terminal. Spectroscopy combined with theory suggests that the solvation of nickel tricarbonyl is dominated by a water-ring network. Here, the present findings would have important implications for the fundamental understanding of the multifaceted mechanisms of the multibody interaction of water and carbon monoxide with transition metals.},
doi = {10.1039/c6cp05035b},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 38,
volume = 18,
place = {United States},
year = {Fri Sep 02 00:00:00 EDT 2016},
month = {Fri Sep 02 00:00:00 EDT 2016}
}
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https://doi.org/10.1039/c6cp05035b
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    Works referencing / citing this record:

    Sulfur substitution in a Ni(cyclam) derivative results in lower overpotential for CO 2 reduction and enhanced proton reduction
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    • Gerschel, P.; Warm, K.; Farquhar, E. R.
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    • DOI: 10.1039/c8dt04740e
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